In situ sol–gel preparation of ZrO2 in nano-composite polymer electrolyte of PVDF-HFP/MG49 for lithium-ion polymer battery

Original Paper: Sol-gel and hybrid materials for energy, environment and building applications

First Online: 07 March 2019

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Abstract

Nano-composite polymer electrolyte (NCPE), poly(vinylidenefluoride-hexafluoropropylene)-poly(methylmethacrylate) grafted natural rubber with lithium tetrafluoroborate and zirconia (PVdF-HFP/MG49-LiBF4-ZrO2) was prepared by a facile one-pot in situ sol–gel method. The influence of zirconia nano-fillers on the electrochemical, chemical and structural properties of polymer electrolyte was investigated. The interaction of polymer electrolyte and zirconia was explored via density functional theory (DFT). Electrochemical impedance spectroscopy study showed that the optimum ionic conductivity is 2.39 × 10−3 S cm−1 (6 wt% zirconia). X-ray diffractogram results revealed a decreasing trend of crystalline phases and no lithium salt peaks were observed upon the addition of zirconia. As a result, the LiBF4 salt was well-solvated in the polymer matrix with a one-fold increase in lithium transference number. Remarkably, a good electrochemical stability was achieved at 6.9 V from a linear sweep voltammetry (LSV) analysis. Observations from the infrared spectra indicate that chemical interactions occurred at the carbonyl and fluoride functional groups and is further corroborated by DFT studies. Micrograph images showed that the zirconia nano-particles were successfully produced (7–15 nm). The nanocomposite polymer electrolyte possesses promising charge/discharge performance and has the potential to be applied in lithium-ion polymer battery.

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Supplementary information

Acknowledgements

The authors would like to acknowledge National University of Malaysia for the research facilities and sponsoring this project under Modal Insan UKM (MI-2018-002 and MI-2018-012) and INOVASI-2017-011. We would also like to thank UKM and Mr. Patrick Tan Sang Hup from KGC Resources Sdn. Bhd. for providing part of the financial support under INOVASI-2017-011. Special thanks to the Japan Student Services Organization (JASSO) for sponsoring the internship program in Japan. Many thanks to Prof. Hideaki Kasai, Prof. Wilson Agerico Diño and Osaka University, Japan for supporting us with the quantum computational facilities.